Biomass Burning in Southern Africa: Individual Particle Characterization of Atmospheric Aerosols and Savanna Fire Samples

Ambient atmospheric aerosols and savanna fireparticulate emission samples from southern Africa werecharacterised in terms of particle classes and theirnumber abundance by electron probe X-ray microanalysis(EPXMA). About ten particle classes were identifiedfor each sample. The major classes werealuminosilicates and sea salts for ambient coarse(2–10 m equivalent aerodynamic diameter (EAD))samples, and K-S and S-only particles for ambient fine(<2 m EAD) samples. The K-S particles are oneof the major products of biomass burning. The EPXMAresults were found to be consistent with the resultsfrom bulk analyses on a sample by sample basis. Forsavanna fire fine samples, quantitative EPXMA revealedthat many particles had a composition of simple saltssuch as KCl. Some particles had a deviatingcomposition in the sense that more ionic species wereinvolved in sustaining the balance between cations andanions, and they were composite or mixed salts.Because of extensive processing during the atmospherictransport, the composition of the K-S particles in theambient samples was different from K₂SO₄,and such particles were enriched with S. The finepyrogenic KCl particles and the fine sea-saltparticles were much depleted in chlorine.     

Continental impact on marine boundary layer coarse particles over the Atlantic Ocean between Europe and Antarctica

Aerosol samples were collected in the Atlantic marine boundary layer between the English Channel and Antarctica during November–December 1999. The composition of coarse (aerodynamic diameter 1–3 μm) individual aerosol particles was studied using the SEM/EDX method. The major particle types observed were fresh sea salt, sea-salt particles reacted partly or totally with sulphuric acid or nitric acid, Mg-sulphate, Ca-sulphate, mixed aluminosilicates and sea salt, aluminosilicates, Ca-rich particles and Fe-rich particles. The relative fractions of sea-salt particles with moderate or strong Cl depletion were high near the coasts of Europe (65–74%) and Northern Africa (44–87%), low far from the coast of Western Africa (10–20%) and very low in remote sea areas between Africa and Antarctica (1%). The Cl depletion was strongest when air masses arrived from the direction of anthropogenic pollution sources. The fractions of Mg-sulphate particles were high (18–25%) in 2 samples near Europe. The Mg-sulphate particles were probably formed as a result of fractional recrystallization of sea-salt particles in which Cl was substituted by sulphate. It remained unclear whether these particles were formed in the atmosphere or during and after sampling. The relative fractions of particles from continental sources were quite low (10–15%) near Europe, very high (25–78%) near the coast of Northwestern Africa and very low in the remote sea areas (0–2%). Most of the continental particles were aluminosilicates and some of them were internally mixed with sea salt. Near the coast of Northwestern Africa, the main source of aluminosilicates was Saharan dust, and near the Gulf of Guinea, emissions from biomass burning were also mixed with aluminosilicates and sea salt.     

Chemical characteristics of haze during summer and winter in Guangzhou

Airborne particles were collected with a 10-stage MOUDI and a PM₁₀ sampler in Guangzhou, China, during both haze and normal days in the summer of 2002 and 2003, and winter 2002. The characteristics of PAHs, organic carbon, elemental carbon and water-soluble inorganic ions were studied under four periods (summer normal, summer haze, winter normal and winter haze). In this study, secondary pollutants (OC, SO₄²⁻, NO₃⁻ and NH₄⁺) were the major chemical components and appeared to show a remarkably rapid increase from normal to haze days. The particle mass size distributions were bimodal and dominated by fine particles in haze days. A significantly higher OC/EC ratio was found in haze days (3.2–4.7) compared to normal days (1.8–2.8), indicating secondary organic aerosol formation might be significant during haze days. Correlation analysis between visibility and chemical species showed that the major scattering species were TC (total carbon) and sulfate in normal days and nitrate and TC in haze days, respectively. Simultaneously, correlation analysis between visibility and meteorological factors demonstrated that visibility increased with both temperature and wind speed, while it decreased with relative humidity. Furthermore, the relatively higher value of IcdP/(BghiP + IcdP) and the low value of Cmax, CPI, and BghiP/BeP in winter haze could be due to the growth of motor vehicle usage and energy consumption in winter.     

Transformation of Aerosol Chemical Properties due to Transport Over a City

The change of the chemical composition of the near-ground level atmospheric aerosol was studied during two summer episodes by a Lagrangian type of experimental approach. Bulk and single-particle chemical analyses of ions and elements in the particulate phase were deployed. N(-III) and N(V) components were also measured in the gas-phase. The measurements were completed by particle size distributions.Secondary inorganic aerosols (SIA) and fine particles of ≈0.2–0.4 μm size were still elevated 50 km downwind of the city. The direct comparison of transport over the city in contrast to transport over the surrounding areas showed that SIA was formed from emission from the city within less than 3 h. Relative increases, i.e., enrichment during transport were observed for primary and secondary aerosol components. The degree of mixing on the individual particle level increased significantly during transport in the area. In particular, newly emitted carbonaceous particles became internally mixed within hours with pre-existing sulphate particles. Mostly due to secondary aerosol formation the average particle size (mass median diameter) of major constituents of the aerosol was significantly decreased while being transported over 13 h. Given recent insights which link fine particles number and mass concentrations with health risks, the results suggest that rural populations in areas which frequently are located within an urban plume might run an elevated health risk relative to populations in areas not affected by urban plumes.     

Concentration and size variation of condensation nuclei at Mawson,Antarctica

Condensation nucleus (CN) concentrations have been measured at Mawson (67.6°S, 62.9°E) since mid 1981. Weekly median concentrations have an annual cycle with a maximum of around 300 to 400 cm^-3 in summer and a minimum of a few tens of particles per cm^-3 in winter. In this respect Mawson behaves very much like an Antarctic continental location. Preliminary measurements of the size distribution of CN particles taken over a nine month period suggest a seasonal change in typical particle radius from around 0.01 m in winter to around 0.04 m in summer. Diurnal variation in the CN concentration is generally very weak and does not show any systematic relation to the pronounced diurnal variation in wind-speed at Mawson.Department of Science, Antarctic Division     

Geochemistry of regional background aerosols in the Western Mediterranean

The chemical composition of regional background aerosols, and the time variability and sources in the Western Mediterranean are interpreted in this study. To this end 2002–2007 PM speciation data from an European Supersite for Atmospheric Aerosol Research (Montseny, MSY, located 40 km NNE of Barcelona in NE Spain) were evaluated, with these data being considered representative of regional background aerosols in the Western Mediterranean Basin. The mean PM₁₀, PM_2.5 and PM₁ levels at MSY during 2002–2007 were 16, 14 and 11 µg/m³, respectively. After compiling data on regional background PM speciation from Europe to compare our data, it is evidenced that the Western Mediterranean aerosol is characterised by higher concentrations of crustal material but lower levels of OM + EC and ammonium nitrate than at central European sites. Relatively high PM_2.5 concentrations due to the transport of anthropogenic aerosols (mostly carbonaceous and sulphate) from populated coastal areas were recorded, especially during winter anticyclonic episodes and summer midday PM highs (the latter associated with the transport of the breeze and the expansion of the mixing layer). Source apportionment analyses indicated that the major contributors to PM_2.5 and PM₁₀ were secondary sulphate, secondary nitrate and crustal material, whereas the higher load of the anthropogenic component in PM_2.5 reflects the influence of regional (traffic and industrial) emissions. Levels of mineral, sulphate, sea spray and carbonaceous aerosols were higher in summer, whereas nitrate levels and Cl/Na were higher in winter. A considerably high OC/EC ratio (14 in summer, 10 in winter) was detected, which could be due to a combination of high biogenic emissions of secondary organic aerosol, SOA precursors, ozone levels and insolation, and intensive recirculation of aged air masses. Compared with more locally derived crustal geological dusts, African dust intrusions introduce relatively quartz-poor but clay mineral-rich silicate PM, with more kaolinitic clays from central North Africa in summer, and more smectitic clays from NW Africa in spring.     

On small particles in the Arctic summer boundary layer: observations at two different heights near Ny-Ålesund, Svalbard

Concurrent observations of particle number densities and size distributions observed at two different heights (near ocean level and 475 m above sea level) in Ny-Ålesund, Svalbard were studied with respect to the diurnal variation during a summer period in June 2004. The results show that observed variation in particle number density in the Arctic boundary layer may be strongly modulated by vertical mixing and dilution. The particles appeared to be formed in the early morning when solar intensity reached about 30% of the mid-day intensity. Based on differences in the observed number densities at the two heights it appears as if particles are formed in the lower part of the boundary layer. The formation rate of 10 nm diameter particles is estimated to be 0.11 cm⁻³ s⁻¹ and the growth rate is in a range between 1 and 2 nm h⁻¹.     

Arctic sea ice and the Madden–Julian Oscillation (MJO)

Arctic sea ice responds to atmospheric forcing in primarily a top-down manner, whereby near-surface air circulation and temperature govern motion, formation, melting, and accretion. As a result, concentrations of sea ice vary with phases of many of the major modes of atmospheric variability, including the North Atlantic Oscillation, the Arctic Oscillation, and the El Niño-Southern Oscillation. However, until this present study, variability of sea ice by phase of the leading mode of atmospheric intraseasonal variability, the Madden–Julian Oscillation (MJO), which has been found to modify Arctic circulation and temperature, remained largely unstudied. Anomalies in daily change in sea ice concentration were isolated for all phases of the real-time multivariate MJO index during both summer (May–July) and winter (November–January) months. The three principal findings of the current study were as follows. (1) The MJO projects onto the Arctic atmosphere, as evidenced by statistically significant wavy patterns and consistent anomaly sign changes in composites of surface and mid-tropospheric atmospheric fields. (2) The MJO modulates Arctic sea ice in both summer and winter seasons, with the region of greatest variability shifting with the migration of the ice margin poleward (equatorward) during the summer (winter) period. Active regions of coherent ice concentration variability were identified in the Atlantic sector on days when the MJO was in phases 4 and 7 and the Pacific sector on days when the MJO was in phases 2 and 6, all supported by corresponding anomalies in surface wind and temperature. During July, similar variability in sea ice concentration was found in the North Atlantic sector during MJO phases 2 and 6 and Siberian sector during MJO phases 1 and 5, also supported by corresponding anomalies in surface wind. (3) The MJO modulates Arctic sea ice regionally, often resulting in dipole-shaped patterns of variability between anomaly centers. These results provide an important first look at intraseasonal variability of sea ice in the Arctic.     

1979~2013年西北太平洋地区海平面气压场季节转换时间的变化分析

采用1979~2013年NCEP/NCAR再分析资料,借助线性趋势、距平、累积距平、Mann-Kendall突变检验及Morlet小波等方法分析了西北太平洋地区海平面气压场季节转换时间的长期趋势和多尺度周期变化特征。结果表明:海平面气压场一年中存在两次季节转变,20°N~50°N海平面气压场冬夏季节转变的时间在第20候左右,而夏冬季节转变发生在第51候。并且海平面气压场的季节转换时间存在纬度差异与经度差异。通过趋势分析,发现海平面气压场由冬季型转变到夏季型的时间存在显著的趋势变化,并且在近35年内是趋于提前,其气候倾向率为-0.33候/10 a;夏季型转换为冬季型的时间趋于延后,气候倾向率为0.25候/10 a。季节转换时间的Mann-Kendall突变检测结果表明,海平面气压场由冬向夏的转换时间在1997~1998年间发生了突变;夏季型转换为冬季型的时间尚未发现显著突变。最后通过对季节转换时间的小波分析与小波功率谱的显著性检验得出,冬夏季节转换的时间具有显著的15 a周期变化;夏冬季节转换时间8 a周期振荡最为剧烈。     

Hygroscopic growth of aerosol particles and its influence on nucleation scavenging in cloud: Experimental results from Kleiner Feldberg

The hygroscopic growth of individual aerosol particles has been measured with a Tandem Differential Mobility Analyser. The hygroscopic growth spectra were analysed in terms of diameter change with increasing RH from 20% to 85%. The measurements were carried out during the GCE cloud experiment at Kleiner Feldberg, Taunus, Germany in October and November 1990.Two groups of particles with different hygroscopic growth were observed. The less-hygroscopic group had average growth factors of 1.11, 1.04 and 1.02 for particle diameters of 50, 150 and 300 nm, respectively. The more-hygroscopic group had average growth factors of 1.34, 1.34, and 1.37 for the same particle diameters. The average fraction of less-hygroscopic particles was about 50%. Estimates of the soluble fractions of the particles belonging to the two groups are reported.Hygroscopic growth spectra for total aerosol, interstitial aerosol and cloud drop residuals were measured. A comparison of these hygroscopic growths of individual aerosol particles provides clear evidence for the importance of hygroscopic growth in nucleation scavenging. The measured scavenged fraction of particles as a function of diameter can be explained by the hygroscopic growth spectra.     

Scavenging of Insoluble Particles from the Marine Atmosphere over the Sub-Arctic North Pacific

Direct deposition measurements ofatmospheric insoluble particles over the sub-ArcticNorth Pacific indicate that the number of particles(6.4 ± 3.8) × 10⁴ cm^-2 per rain eventwas fairly constant compared with the large variationof the precipitation rate, which ranged from 0.16 to18 mm per event for 43 rain days during the period ofMarch–September (total 109 days) 1996. Thissuggests that insoluble particles larger than 0.4 min area equivalent diameter are primarilyremoved at the margin of the rainfall area by wetscavenging processes below clouds in the marineatmosphere in sub-Arctic regions. The frequency ofrain events controls the fate of the troposphericaerosols larger than sub-micrometer in diameter. Reflecting the seasonal long-range transport of Asiandust, mineral particles were dominant as insolubleparticles in the spring rains, but carbonaceousparticles were dominant in the summer rains. Theatmospheric deposition of insoluble particles could besignificant as a source of sediment particles over thesub-Arctic North Pacific.     

Vertical Distribution Characteristics of PM<Subscript>2.5</Subscript> Observed by a Mobile Vehicle Lidar in Tianjin,China in 2016

We present mobile vehicle lidar observations in Tianjin, China during the spring, summer, and winter of 2016. Mobile observations were carried out along the city border road of Tianjin to obtain the vertical distribution characteristics of PM_2.5. Hygroscopic growth was not considered since relative humidity was less than 60% during the observation experiments. PM_2.5 profile was obtained with the linear regression equation between the particle extinction coefficient and PM_2.5 mass concentration. In spring, the vertical distribution of PM_2.5 exhibited a hierarchical structure. In addition to a layer of particles that gathered near the ground, a portion of particles floated at 0.6–2.5-km height. In summer and winter, the fine particles basically gathered below 1 km near the ground. In spring and summer, the concentration of fine particles in the south was higher than that in the north because of the influence of south wind. In winter, the distribution of fine particles was opposite to that measured during spring and summer. High concentrations of PM_2.5 were observed in the rural areas of North Tianjin with a maximum of 350 μg m^–3 on 13 December 2016. It is shown that industrial and ship emissions in spring and summer and coal combustion in winter were the major sources of fine particles that polluted Tianjin. The results provide insights into the mechanisms of haze formation and the effects of meteorological conditions during haze–fog pollution episodes in the Tianjin area.     

Role of the volatile fraction of submicron marine aerosol on its hygroscopic properties

The hygroscopic growth factor (HGF) of 85 nm and 20 nm marine aerosol particles was measured during January 2006 for a three-week period within the frame of the EU FP6 project MAP (Marine Aerosol Production) winter campaign at the coastal site of Mace Head, using the TDMA technique. The results are compared to aerosol particles produced in a simulation tank by bubbling air through sea water sampled near the station, and through synthetic sea water (inorganic salts). This simulation is assimilated to primary production. Aitken and mode particles (20 nm) and accumulation mode particles (85 nm) both show HGF of 1.92 and 2.01 for particles generated through bubbling in natural and artificial sea water respectively. In the Aitken mode, the marine particles sampled in the atmosphere shows a monomodal HGF slightly lower than the one measured for sea salt particles artificially produced by bubble bursting in natural sea water (HGF = 1.83). This is also the case for the more hygroscopic mode of accumulation mode particles. In addition, the HGF of 85 nm particles observed in the atmosphere during clean marine sectors exhibits half of its population with a 1.4 HGF. An external mixture of the accumulation mode marine particles indicates a secondary source of this size of particles, a partial processing during transport, or an inhomogeneity of the sea water composition. A gentle 90 °C thermo-desorption results in a significant decrease of the number fraction of moderately hygroscopic (HGF = 1.4) particles in the accumulation mode to the benefit of the seasalt mode, pointing to the presence of semi-volatile compounds with pronounced hydrophobic properties. The thermo-desorption has no effect on the HGF of bubble generated aerosols, neither for synthetic or natural sea water, nor on the atmospheric Aitken mode, indicating that these hydrophobic compounds are secondarily integrated in the particulate phase. No difference between night and day samples is observed on the natural marine aerosols regarding hygroscopicity, but a more pronounced sensitivity to volatilization of the 1.4 HGF mode in the accumulation mode is observed during the day.     

Atmospheric circulation characteristics during some El-Nino years in relation to Indian summer monsoon rainfall

Summary Based on observed rainfall data of India Meteorological Department (IMD), correlation coefficients (CCs) have been computed between Indian summer monsoon rainfall (ISMR) and sea surface temperature (SST) anomalies over different Nino regions and standardised pressure difference between Tahiti and Darwin. Significant positive CCs are found between the Southern Oscillation Index (SOI) in winter and subsequent June rainfall over India. Concurrent with and subsequent to Indian summer monsoon, SOI shows significant positive CC with the mean rainfall of July to September (JAS). Significant negative CCs are found between JAS mean rain and the concurrent and following SST anomalies over Nino-3.4 region. On the basis of these correlations, it is proposed that the entire period of summer monsoon from June to September could be divided into two sub-periods such as: early summer (June) and mid-late summer (July to September) monsoon for prediction of ISMR in the extended range.In order to examine the characteristics of atmospheric circulation during some El-Nino years, divergent flow at 200hPa and omega field at 500hPa based on NCEP/NCAR reanalysis have been studied in detail. Major significant southward shift of upper level divergent field from India are related to El-Nino and this shift may be responsible for causing droughts during several El-Nino years over India. Also vertical wind fields at 500hPa show sinking motion over large parts of India and west Pacific and ascending motion over southern Indian Ocean, central and eastern Pacific during major drought years.     

State of mixing, shape factor, number size distribution, and hygroscopic growth of the Saharan anthropogenic and mineral dust aerosol at Tinfou, Morocco

The Saharan Mineral Dust Experiment (SAMUM) was conducted in May and June 2006 in Tinfou, Morocco. A H-TDMA system and a H-DMA-APS system were used to obtain hygroscopic properties of mineral dust particles at 85% RH. Dynamic shape factors of 1.11, 1.19 and 1.25 were determined for the volume equivalent diameters 720, 840 and 960 nm, respectively.
During a dust event, the hydrophobic number fraction of 250 and 350 nm particles increased significantly from 30 and 65% to 53 and 75%, respectively, indicating that mineral dust particles can be as small as 200 nm in diameter. Log-normal functions for mineral dust number size distributions were obtained from total particle number size distributions and fractions of hydrophobic particles. The geometric mean diameter for Saharan dust particles was 715 nm during the dust event and 570 nm for the Saharan background aerosol.
Measurements of hygroscopic growth showed that the Saharan aerosol consists of an anthropogenic fraction (predominantly non natural sulphate and carbonaceous particles) and of mineral dust particles. Hygroscopic growth and hysteresis curve measurements of the 'more' hygroscopic particle fraction indicated ammonium sulphate as a main component of the anthropogenic aerosol. Particles larger than 720 nm in diameter were completely hydrophobic meaning that mineral dust particles are not hygroscopic.     

Ice-Core Study of the Link between Sea-Salt Aerosol,Sea-Ice Cover and Climate in the Antarctic Peninsula Area

Three ice cores and a set of snow pit samples collected on James Ross Island, Antarctic Peninsula, in 1979, 1981 and 1991 have been analyzed for water stable isotope content D or ¹⁸O (isotopic temperature) and major chemical species. A reliable and detailed chronological scale has been established first for the upper 24.5 m of water equivalent (1990–1943) where various data sets can be compared, then extended down to 59.5 m of water equivalent (1847) with the aid of seasonal variations and the sulphate peak reflecting the 1883 Krakatoa volcanic eruption. At James Ross Island, sea-salt aerosol is generally produced by ice-free marine surfaces during the summer months, although some winter sea-salt events have been observed. For the upper part of the core (1990–1943), correlations (positive or negative) were calculated between isotopic temperature, chloride content (a sea-salt indicator), sea-ice extent, regional atmospheric temperature changes and atmospheric circulation. The D and chloride content correlation was then extended back to 1847, making it possible to estimate decadal sea-ice cover fluctuations over the study period. Our findings suggest that ice-core records from James Ross Island reflect the recent warming and sea-ice decrease trends observed in the Antarctic Peninsula area from the mid-1940s.     

Source attribution of urban smog episodes caused by coal combustion

Stable weather conditions together with extensive use of coal combustion often lead to severe smog episodes in certain urban environments, especially in Eastern Europe. In order to identify the specific sources that cause the smog episodes in such environments, and to better understand the mixing state and atmospheric processing of aerosols, both single particle and bulk chemical characterization analysis of aerosols were performed in Krakow, Poland, during winter 2005.Real-time measurements of the bulk PM10 aerosol during a severe smog episode (PM10 mass > 400 µg m^− 3) showed a stable concentration of black carbon in the aerosol, and an increase in the sulphate and chlorine mass contributions towards the end of the episode. Chemical characterization of single particles further helped to identify residential coal burning as the main source that caused this severe smog episode, consisting of single particles with major signals for carbon with simultaneous absence of sulphate, chlorine and calcium. Particles from industrial coal combustion gained importance towards the end of that episode, after residential coal combustion was switched off, indicated by an increase of the percentage of sulphate and chlorine containing particles. Traffic was not a significant source during the severe smog episode. During a lighter smog episode, residential and industrial coal combustion was still predominant, with an increased contribution of traffic and processed/aged aerosols. On a clean day, particle classes containing nitrate were the most abundant. In addition, the aerosol was more internally mixed showing that there were more sources contributing to the total aerosol population.     

Distribution of nitrate over sea-salt and soil derived particles — Implications from a field study

A method for determining the distribution of supermicrometer nitrate between size-segregated sea-salt and soil derived particles is presented. The analysis is based on field data from six measurements at a coastal site in southern Finland, and on a theoretical treatment taking into account the transfer of gaseous species onto particle surfaces and their subsequent reaction. Significant amounts of nitrate were found in both the particle types, with the fraction of nitrate associated with soil particles varying from 20–50% in the 1–2 m size to near 90% in particles larger than 10 m. Overall, the nitrate accumulation followed closely the relative abundances of these two particle types. Two overlapping modes in supermicron nitrate mass size distributions could be identified. The lower mode, associated with sea-salt, was located between the surface-area and volume distribution of sodium peaking at about 2–3 m of EAD. The upper mode peaked at 3–5 m and followed more closely the surface-area distribution of calcium in all samples. At our site, the accumulation of nitrate into both particle types was shown to be limited by an effective surface reaction rate rather than by gas-phase diffusion. This rate was estimated to be considerably larger for sea-salt particles. Strong evidence in support of the saturation of nitrate in sea-salt particles were obtained.     

Evolution of boundary‐layer aerosol particles due to in‐cloud chemical reactions during the 2nd Lagrangian experiment of ACE‐2

The second Aerosol Characterisation Experiment (ACE‐2) was aimed at investigating the physical, chemical and radiative properties of aerosol and their evolution in the North Atlantic region. In the 2nd "Lagrangian" experiment, an air mass was tracked over a 30‐h period during conditions of extensive stratocumulus cover. Boundary‐layer measurements of the aerosol size distribution obtained with a passive cavity aerosol spectrometer probe (PCASP) during the experiment show a gradual growth in size of particles in the 0.1–0.2 μm diameter mode. Simultaneously, SO₂ concentrations were found to decrease sharply from 800 to 20 ppt. The fraction of sulphate in aerosol ionic mass increased from 0.68±0.07 to 0.82±0.09 for small particles (diameter below 1.7 μm) and from 0.21±0.04 to 0.34±0.03 for large particles (diameter above 1.7 μm). The measurements were compared with a multicyclic parcel model of gas phase diffusion into cloud droplets and aqueous phase chemical reactions. The model was able to broadly reproduce the observed transformation in the aerosol spectra and the timescale for the transformation of SO₂ to sulphate aerosol. The modelled SO₂ concentration in the boundary layer fell to below half its initial value over a 6.5‐h time period due to a combination of the entrainment of cleaner tropospheric air and cloud chemical reactions. NH₃ and HCl gas were also found to play an important rôle in cloud processing in the model.     

Formate and acetate levels compared in monsoon and winter rainwater at Dayalbagh, Agra (India)

A total of 59 rainwater samples were collected during the winter and monsoon (1991–92) at Dayalbagh, Agra. This site is relatively free from the influence of anthropogenic emissions and the volume-weighted average concentrations (VWA) of formate in the winter and monsoon were 22.5±6, 16.1±3 while acetate VWAs were 17.1±5 and 13.8±3 mol l^-1, respectively. Although the VWAs varied between seasons, it was not statistically different. Total deposition (in mmol m^-2) varied between season (winter formate, 1.4; acetate, 1.1; monsoon formate, 7.4; acetate, 6.4). A difference in VWA values may have occurred as a result of the dilution factor; the total rain depth from collected samples in the monsoon was 46 cm while that in winter was 6.3 cm. Sources at this site may be anthropogenic and natural; scavenging from the vapour phase, washout of soil particles and emissions from vegetative sources are probably important sources for formate and acetate.